Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard

Aerosol–cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice-nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because INPs and INMs have spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nuclei Counter (FINC) for the estimation of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous droplet freezing techniques (DFTs) and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.4 ± 0.2 ∘C with 5 µL, and has an instrument temperature uncertainty of ± 0.5 ∘C. We further conducted freezing control experiments to quantify the nonhomogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample from two other drop freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and the University of Basel's LED-based Ice Nucleation Detection Apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice-nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we compared lignin's freezing temperature across different drop freezing instruments, including on DRINCZ and LINDA, and then determined an empirical fit parameter for future drop freezing validations. Subsequently, we showed that commercial lignin has consistent ice-nucleating activity across product batches and demonstrated that the ice-nucleating ability of aqueous lignin solutions is stable over time. With these findings, we present lignin as a good immersion freezing standard for future DFT intercomparisons in the research field of atmospheric ice nucleation.

Monitoring ambient aerosol size distributions from 1 – 55 nm with the GRIMM-AIRMODUS PSMPS

<p>Here, we present the final, commercially available, version of a mobility particle size spectrometer that is able to access the 1 nm particle size range for ambient atmospheric measurements.</p><p>The overall system performance was tested in a multitude of laboratory experiments, determining various size dependent parameters like DMA’s transfer function, DMA penetration efficiency, PSM and CPC counting efficiency. With the knowledge of these parameters, we are able to define a well-known overall system performance, a critical prerequisite for measurements that start at 1 nm sized particles.</p><p>The instrument originates from a collaboration of Grimm Aerosol Technik, Germany and Airmodus Ltd, Finland, combining a Grimm SMPS+C system with the Airmodus Particle Size Magnifier (PSM). Accordingly, it is named: PSMPS.</p><p>The main system components comprise a modified version of the short Grimm Differential Mobility Analyzer (Grimm S-DMA), the diethylene glycol-based PSM (Airmodus A10) and the new butanol-based CPC (Grimm 5417). The modified S-DMA is specially optimized for the transmission of small ions. Typically, it is operated with an aerosol sample flow rate of 2.5 L/min and a sheath flow rate of 10 L/min, allowing particle size distribution measurements from 1.1-55.7 nm. The PSM is used to lower the detection efficiency of the Grimm CPC below 2 nm in electrical mobility equivalent diameter. The new Grimm 5417 CPC is an upgraded version of the well-known 5416 CPC, that features two switchable aerosol sample flow rates of 0.3 and 0.6 L/min and also supplies the S-DMA with sheath airflow rates of either 3.0 or 10.0 L/min.</p><p>In this presentation, we will introduce the features and performance of the PSMPS system, will highlight some laboratory characterization tests and report the results from an ambient aerosol measurement campaign at the Hohenpeissenberg Observatory of the German meteorological service (DWD), monitoring new particle formation events starting at a particles size of 1nm.</p>

Сomparative analysis of disperse characteristics of single-type flat spray cone nozzles

Research and development work related to the study and use of water spray must certainly be based on the most accurate determination of the dispersion composition of spray droplets. It is just this parameter that forms the basis for all further calculations of the effect of water spray on the process cycle components. The introduction of the method for restoring the original sizes of spray droplets and the most accurate measurement of their disperse characteristics will allow coming close to solving the problem of optimizing the operation of spray technology, as well as will make it possible to predict and possibly regulate the dispersed characteristics of droplet flows. Therefore, it is the foundation for the development of breakthrough and environmentally sustainable resource-saving technologies in the agricultural sector. We have developed a method for restoring the original size of the droplet spectrum (Patent No. 2709402 titled “A method for determining the size of droplets”). Based on this method, a test bench was developed and manufactured to assess the quality of spraying of working fluids. An aerosol chamber design was developed and the chamber was assembled, in which an aerosol sample was taken under conditions of equal probability of deposition and preservation of droplets of all sizes. Software for high-speed measurement of the dispersion characteristics of the spectrum of spray droplets has been developed. In general, the studies performed have demonstrated the appropriate professional capabilities of the experimental facilities when testing sprayers. This gives us an opportunity to come up with a proposal to create centers for testing sprayers for their compliance with the declared performances based on the experimental facilities.

Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard

Aerosol-cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because of INPs' and INMs' spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge, requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nucleation Counter (FINC), a droplet freezing technique (DFT), for the quantification of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous DFTs and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 μL volume, has a limit of detection of −25.37 ± 0.15 °C with 5 μL, and has an instrument temperature uncertainty of ±0.5 °C. We further conducted freezing control experiments to quantify the non-homogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample with two other drop-freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and University of Basel's LED-based ice nucleation detection apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we compare its freezing temperature across different drop-freezing instruments, including on DRINCZ and LINDA, and determine an empirical fit parameter for future drop freezing validations. Second, we show that commercial lignin has a consistent ice nucleating activity across product batches. Third, we demonstrate that the ice nucleating ability of aqueous lignin solutions are stable over time. With these findings, we aim to show that lignin can be used as a good immersion freezing standard in future technique intercomparisons in the field of atmospheric ice nucleation.

Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard

Aerosol-cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because of INPs' and INMs' spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge, requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nucleation Counter (FINC), a droplet freezing technique (DFT), for the quantification of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous DFTs and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.37 ± 0.15 ˚C with 5 µL, and has an instrument temperature uncertainty of ± 0.5 ˚C. We further conducted freezing control experiments to quantify the non-homogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample with two other drop-freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and University of Basel’s LED-based ice nucleation detection apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we show that commercial lignin has a consistent ice nucleating activity across product batches. Second, we demonstrate that aqueous lignin solutions exhibit good solution stability over time. Third, we compare its freezing temperature across different drop-freezing instruments, including on DRINCZ, LINDA, and on the Weizmann Institute's Supercooled Droplets Observation on a Microarray (WISDOM) and determine an empirical fit parameter for future drop freezing validations. With these findings, we aim to show that lignin can be used as a good immersion freezing standard in future technique intercomparisons in the field of atmospheric ice nucleation.

Evaluation of combined radiocarbon and carbon stable isotope data of PM2.5 carbonaceous aerosol in Debrecen, Hungary

<p>Comprehensive atmospheric studies have demonstrated that carbonaceous aerosol is one of the main components of atmospheric particulate matter over Europe. Despite its significant role in atmospheric processes, the characteristic of carbonaceous particle sources and the contributions from modern and fossil sources in the Pannonian Basin are still less known. Using radiocarbon as a tracer, the ratio of modern (biological aerosol, wood burning etc.) and fossil (coal or oil burning, transportation) sources for an aerosol sample can unambiguously be determined but identification of exact sources is not possible. Considering other isotopic techniques, carbon stable isotope results can provide us such supplementary information that can be used in separating different large source clusters (e.g. burning of C3 type wood, coal burning or transportation). Different aerosol sources have well defined carbon stable isotope ranges, which can be used in source apportionment models. Nevertheless, these ranges often overlap each other, making the accurate source identification rather difficult. Combined radiocarbon and carbon stable isotope measurements can however help us to differentiate more precisely numerous modern or fossil sources.</p><p>In our study, the isotopic composition of carbon in the PM<sub>2.5 </sub>atmospheric aerosol collected on weekly basis in Debrecen, Hungary was investigated. In doing so, the organic and elemental carbon content, the specific <sup>14</sup>C content and the δ<sup>13</sup>C values of total carbon were measured using a Sunset OC/EC analyser, an accelerator mass spectrometer (AMS) and an EA/IRMS instrument, respectively. Based on our three-year long carbon stable isotope data of carbonaceous aerosol, relatively enriched δ<sup>13</sup>C results can be observed in each wintertime period, which are supposed by other authors to be related to the effect of coal combustion (mainly in heavily industrialised areas). Contrarily, radiocarbon measurements imply the dominance of modern sources for the same wintertime periods when the biological activity of vegetation is moderate. Consequently, according to our assumption, these values are caused by modern sources having more positive δ<sup>13</sup>C value such as biomass burning of residences. In contrast to single stable isotope or radiocarbon measurements our study sheds light on the importance of combined carbon isotopic investigations. The research was supported by the European Union and the State of Hungary, co-financed by the European Regional Development Fund in the project of GINOP-2.3.2-15-2016-00009 ‘ICER’</p>

Iodine speciation and size distribution in ambient aerosols at a coastal new particle formation hotspot in China

Intense new particle formation (NPF) events were observed in the coastal atmosphere during algae growth and farming season at Xiangshan gulf of the east China coast. High nucleation-mode iodine concentrations measured by ultra-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry (UPLC/Q-TOF-MS) confirmed that the NPF events were induced by iodine species. Our study provides important information on iodine speciation, size distributions, and its role in NPF in the context of heavy air pollution in China's coastal areas. For the first time, we identified 5 inorganic iodine species, 45 organic iodine compounds (35 molecular formulas), and a group of iodide–organic adducts in aerosols. The concentrations and size distributions of iodine species down to 10 nm were measured during the iodine-induced NPF, continental NPF, and non-NPF days at the coastal site and compared to those at an inland site. The iodine in the above four aerosol sample types were characterized by iodate, aromatic iodine compounds, iodoacetic acid or iodopropenoic acid, and iodide–organic adducts, respectively. Iodide and organic iodine compounds were found in the nucleation-mode particles; however, it is still not clear whether they contributed to nucleation or just new particle growth. Wild algae, as well as farmed algae, could be an important NPF source in China's coastal areas.

Diagnostics of Plasma Pencil Discharge for Chemical Analysis

We present diagnostics of plasma pencil discharge as alternative excitation source for analytical chemistry. The plasma pencil is special type of rf plasma nozzle at atmospheric pressure. Through this nozzle flows working gas argon with aerosol. The aerosol sample introduction system employed a double pass Scott spray chamber with a pneumatic concentric nebulizer. The parameters of the plasma were calculated by optical emission spectroscopy.<br /><br />